The invention discloses carbon nanotube/polypyrrole nanotube composite electronic ink and a preparation method thereof, and relates to an electronic ink technology. The electronic ink is mainly prepared from, by weight, 0.4-1.2 parts of polypyrrole nanotube, 0.4-1.2 parts of carbon nanotubes, 1.2-4.8 parts of bacterial cellulose, 0.4-1.2 parts of a surface active agent, 0.2-0.6 part of carboxymethylcellulose, 0.4-1.2 parts of a color-fixing agent, 2-6 parts of 3-amidogen propyl triethoxysilane, 10-20 parts of ethyl alcohol, 50 parts of deionized water and 40 parts of 1-methyl-2-pyrrolidone. The electrical conductivity of polypyrrole powder obtained through freezing interface polymerization is high, and the polypyrrole powder can be taken as a nanomaterial of the electronic ink. After polypyrrole is modified through bacterial cellulose, the obtained dispersion liquid is more uniform, the phenomenon of precipitation and gathering cannot easily occur, and addition of the color-fixing agent, the carboxymethylcellulose and the 3-amidogen propyl triethoxysilane can improve the binding force between ink and basic materials. After the prepared ink is subjected to silk-screen printing, a coating with washable performance and higher electrical conductivity can be obtained, in the process of preparing the ink, conditions are controllable, and the cost is lower.